CN102479973B - Silicon cathode lithium ion battery - Google Patents
Silicon cathode lithium ion battery Download PDFInfo
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- CN102479973B CN102479973B CN201110078105.5A CN201110078105A CN102479973B CN 102479973 B CN102479973 B CN 102479973B CN 201110078105 A CN201110078105 A CN 201110078105A CN 102479973 B CN102479973 B CN 102479973B
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- ion battery
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0568—Liquid materials characterised by the solutes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0569—Liquid materials characterised by the solvents
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention provides a silicon cathode lithium ion battery which comprises a shell, an electric core and a non-aqueous electrolyte which are accommodated in the shell, wherein the electric core comprises an anode, a silicon cathode and a diaphragm arranged between the anode and the silicon cathode; the non-aqueous electrolyte comprises a lithium salt, a non-aqueous solvent and an additive; and the additive contains diallyl pyrocarbonate. In the silicon cathode lithium ion battery, the diallyl pyrocarbonate is adopted in the non-aqueous electrolyte, a stable SEI membrane is formed between the non-aqueous solvent and lithium ions, and a reaction between a Li-Si alloy and an organic solvent is released and inhibited, therefore, charge and discharge properties of the silicon cathode lithium ion battery are effectively improved, side reactions are reduced, battery inflation is reduced, and cycle life of the battery is prolonged.
Description
Technical field
The invention belongs to field of lithium ion battery, particularly relate to a kind of silicon cathode lithium ion battery.
Background technology
Adopt cobalt acid lithium, lithium nickelate, LiMn2O4 or LiFePO4 to have that operating voltage is high, specific energy is large as the lithium ion battery of positive electrode, pollution-free, memory-less effect and the advantage such as the life-span is long, be widely used in the portable electric apparatuses such as mobile phone, digital camera and notebook computer, simultaneously as the alternative energy source of oil in electric motor car and hybrid electric vehicle also by large-scale application.Silicon materials have larger lithium storage content, and enrich content in the earth, are the desirable negative material of lithium ion battery.
Adopt silicon materials as the negative pole of lithium ion battery, in battery charging and discharging cyclic process, the reversible generation of Li-Si alloy and decomposition are along with huge change in volume, efflorescence or the crack of alloy can be caused, cause peeling off of the avalanche of silicon material structure and electrode material, and make electrode material lose electrical contact, cause the cycle performance of silicon cathode lithium ion battery sharply to decline.Simultaneously due to the generation of side reaction, a large amount of gas can be produced in charge and discharge process, easy inside battery flatulence.
At present for promoting the efficiency for charge-discharge of silicium cathode material lithium ion battery, mainly to change the master that consists of of battery pole piece, such as, can improve the content of amorphous silicon in electrode material or adopt the silicon materials of carbon film coated.Such as, disclose a kind of lithium battery in CN101685875A, comprise silicium cathode, lithium metal mixing oxide and barrier film, the electrolyte solution that this lithium battery adopts comprises organic solvent, lithium salts, additive, the copolymer containing maleimide, bismaleimides, poly maleimide, polybismaleimide, bismaleimides and maleimide in additive and vinylene carbonate.But the efficiency for charge-discharge of this lithium battery is still lower, because inside battery flatulence causes the life-span of battery lower.
Summary of the invention
The invention solves the efficiency for charge-discharge of the silicon cathode lithium ion battery existed in prior art and life-span low technical problem.
The invention provides a kind of silicon cathode lithium ion battery, comprise housing and be contained in battery core, the nonaqueous electrolytic solution in housing, battery core comprises positive pole, silicium cathode and the barrier film between positive pole and silicium cathode; Described nonaqueous electrolytic solution comprises lithium salts, nonaqueous solvents and additive, containing coke diene acid propyl diester in described additive.
Silicon cathode lithium ion battery provided by the invention, by adopting coke diene acid propyl diester in nonaqueous electrolytic solution, stable SEI film is formed between nonaqueous solvents and lithium ion, the reaction alleviate, suppressed between Li-Si alloy and organic solvent, thus effectively improve the charge-discharge performance of silicon cathode lithium ion battery, reduce the generation of side reaction, thus reduce battery flatulence, improve the cycle life of silicon cathode lithium ion battery.
Embodiment
The invention provides a kind of silicon cathode lithium ion battery, comprise housing and be contained in battery core, the nonaqueous electrolytic solution in housing, battery core comprises positive pole, silicium cathode and the barrier film between positive pole and silicium cathode; Described nonaqueous electrolytic solution comprises lithium salts, nonaqueous solvents and additive, containing coke diene acid propyl diester in described additive.
Silicon cathode lithium ion battery provided by the invention, by adopting coke diene acid propyl diester in nonaqueous electrolytic solution, the structural formula of described coke diene acid propyl diester is
; Wherein burnt carbonate structural can effectively promote to form stable SEI film between nonaqueous solvents and lithium ion, the reaction alleviate, suppressed between Li-Si alloy and organic solvent, thus effectively improves the charge-discharge performance of silicon cathode lithium ion battery; On the other hand, C=C double bond structure in pi-allyl can consume the moisture in electrolyte on the one hand, improve charge-discharge performance, the micro-HF in electrolyte can be consumed on the other hand, avoid the reaction of HF and SEI film, effectively can reduce the generation of side reaction, avoid inside battery flatulence, therefore effectively can improve the cycle life of battery.
The nonaqueous electrolytic solution of silicon cathode lithium ion battery of the present invention, suppresses the reaction of Li-Si alloy and organic solvent, thus effectively can improve the charge-discharge performance of silicon cathode lithium ion battery mainly through coke diene acid propyl diester.Do not adopt silicon materials as the lithium ion battery of negative pole for other, the charge-discharge performance impact of coke diene acid propyl diester on battery is little.
In silicon cathode lithium ion battery of the present invention, in nonaqueous electrolytic solution, the content of coke diene acid propyl diester is without the need to too high, can improve charge-discharge performance and the cycle life of lithium ion battery.Particularly, with the nonaqueous electrolytic solution of 100 weight portions for benchmark, the content of coke diene acid propyl diester is 0.1-10 weight portion.
In electrolyte of the present invention, the content of lithium salts and nonaqueous solvents is not specially required, in the usual range of the art.Particularly, with the nonaqueous electrolytic solution of 100 weight portions for benchmark, the content of lithium salts is 1-10 weight portion, and the content of nonaqueous solvents is 80-98.9 weight portion.
Described lithium salts is the various lithium salts that those skilled in the art commonly use, such as, can be selected from lithium perchlorate (LiClO
4), lithium hexafluoro phosphate (LiPF
6), LiBF4 (LiBF
4), hexafluoroarsenate lithium (LiAsF
6), LiSO
3f, LiCF
3sO
3in at least one.
In the present invention, the various nonaqueous solventss that described nonaqueous solvents adopts those skilled in the art to commonly use.Such as, at least one in vinyl carbonate (EC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), ethylene fluoride carbonic ether (FEC), diethyl carbonate (DEC) can be selected from.
Can also containing pyrocarbonic acid diethyl ester and/or coke acid di-t-butyl ester in additive of the present invention.With the nonaqueous electrolytic solution of 100 weight portions for benchmark, the content of pyrocarbonic acid diethyl ester is 0.1-10 weight portion, and the content of coke acid di-t-butyl ester is 0.1-10 weight portion.
In silicon cathode lithium ion battery of the present invention, the encapsulating structure of the structure of positive pole, barrier film, material and battery is conventionally known to one of skill in the art, repeats no more in the present invention.The negative pole of the silicon cathode lithium ion battery in the present invention is silicium cathode, and described silicium cathode can adopt silicon nanowire material.For improve silicon materials electrical conductivity, avoid silicon materials surface to react with nonaqueous electrolytic solution time produce loss of capacitance compared with high irreversible, the silicon nanowire material that described silicium cathode can adopt carbon coated.
Below in conjunction with embodiment, silicon cathode lithium ion battery of the present invention is described further.In embodiment and comparative example adopt and be all commercially available.
Embodiment 1
1. the preparation of nonaqueous electrolytic solution
At room temperature, in the glove box of water content < 5ppm, vinyl carbonate (EC), diethyl carbonate (DEC) and ethyl methyl carbonate (EMC) are mixed as nonaqueous solvents, by the LiPF of 8 weight portions by weight 2:1:3
6be dissolved in the nonaqueous solvents of 87 weight portions, then add the coke diene acid propyl diester of 5 weight portions, obtain the nonaqueous electrolytic solution of the present embodiment, be designated as S1.
2. silicium cathode lithium-ion button battery makes
By LiCoO
2, PVDF(Kynoar), conductive agent suppresses on aluminium foil after mixing, and obtains positive plate; By silicon nanowire material, CMC(Carboxylic Acid Fibre element sodium), SBR(butadiene-styrene rubber) mix after suppress on Copper Foil, obtain negative plate; Barrier film is PE/PP composite diaphragm, adopts the nonaqueous electrolytic solution S1 that step 1 is obtained, adopts normal battery process to be made into silicium cathode lithium-ion button battery A1 in argon gas glove box.
Comparative example 1
Adopt the method identical with embodiment 1 to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery, difference is: in step 1, directly by the LiPF of 8 weight portions
6be dissolved in the nonaqueous solvents of 92 weight portions, after mixing, obtain the nonaqueous electrolytic solution DS1 of this comparative example.By the step 2 identical with embodiment 1, obtain silicium cathode lithium-ion button battery DA1.
Comparative example 2
Adopt the method identical with embodiment 1 to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery, difference is: in step 1, by the LiPF of 8 weight portions
6be dissolved in the nonaqueous solvents of 89.50 weight portions, then add the pyrocarbonic acid diethyl ester of 0.5 weight portion and the vinylene carbonate of 2 weight portions, obtain the nonaqueous electrolytic solution DS2 of this comparative example.By the step 2 identical with embodiment 1, obtain silicium cathode lithium-ion button battery DA2.
Embodiment 2
Adopt the method identical with embodiment 1 to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery, difference is: in step 1, by the LiPF of 9 weight portions
6be dissolved in the nonaqueous solvents of 91.9 weight portions, then add the coke diene acid propyl diester of 0.1 weight portion, obtain the nonaqueous electrolytic solution S2 of the present embodiment.By the step 2 identical with embodiment 1, obtain silicium cathode lithium-ion button battery A2.
Embodiment 3
Adopt the method identical with embodiment 1 to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery, difference is: in step 1, by the LiPF of 4 weight portions
6be dissolved in the nonaqueous solvents of 86 weight portions, then add the coke diene acid propyl diester of 10 weight portions, obtain the nonaqueous electrolytic solution S3 of the present embodiment.By the step 2 identical with embodiment 1, obtain silicium cathode lithium-ion button battery A3.
Embodiment 4
Adopt the method identical with embodiment 1 to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery, difference is: in step 1, by the LiPF of 5 weight portions
6be dissolved in the nonaqueous solvents of 85 weight portions, then add the coke acid di-t-butyl ester of the coke diene acid propyl diester of 4 weight portions, the pyrocarbonic acid diethyl ester of 3 weight portions and 3 weight portions, obtain the nonaqueous electrolytic solution S4 of the present embodiment.By the step 2 identical with embodiment 1, obtain silicium cathode lithium-ion button battery A4.
Embodiment 5-8
The method identical with embodiment 1-4 is adopted to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery respectively, difference is: in step 2, silicon nanowire material in the silicon nanowire material difference alternate embodiment 1-4 adopting carbon coated, obtains silicium cathode lithium-ion button battery A5-A8 successively.
Comparative example 3-4
The method identical with comparative example 1-2 is adopted to prepare positive pole, negative pole, nonaqueous electrolytic solution and silicon cathode lithium ion battery respectively, difference is: in step 2, the silicon nanowire material adopting carbon coated substitutes the silicon nanowire material in comparative example 1-2 respectively, obtains silicium cathode lithium-ion button battery DA3-DA4 successively.
Embodiment 9-12
Adopt the method identical with embodiment 1-4 step 1 to prepare nonaqueous electrolytic solution respectively, then nonaqueous electrolytic solution is injected aluminum hull rectangular cell respectively, the positive electrode of aluminum-shell battery adopts LiCoO
2, negative material adopts the coated silicon nanowire material of carbon, obtains silicium cathode lithium ion aluminum-shell battery A9-A12 after assembling successively.
Comparative example 5-6
Adopt the method identical with comparative example 1-2 step 1 to prepare nonaqueous electrolytic solution respectively, then nonaqueous electrolytic solution is injected aluminum hull rectangular cell respectively, the positive electrode of aluminum-shell battery adopts LiCoO
2, negative material adopts the coated silicon nanowire material of carbon, obtains silicium cathode lithium ion aluminum-shell battery DA5-DA6 after assembling successively.
Performance test:
(1) respectively with the electric current of 0.1mA, charge and discharge cycles test is carried out to silicium cathode lithium-ion button battery A1-A8 and DA1-DA4, voltage is 0.005V-1.5V, the charging capacity of record battery and discharge capacity, calculate discharging efficiency (%)=charging capacity/discharge capacity × 100%.Test result is as shown in table 1.
(2) carry out charge and discharge cycles test to silicium cathode lithium ion aluminum-shell battery A9-A12 and DA5-DA6 with the electric current of 200mA respectively, voltage is 3.0V-4.2V, record initial charge capacity and discharge capacity, calculates discharging efficiency (%); Circulate after 100 times, record residue charge/discharge capacity, socking out capacity/discharge capacity × 100% first after capacity surplus ratio (%)=circulation 100 times after computation cycles; And the thickness recorded before and after aluminum-shell battery circulation.Test result is as shown in table 2.
Table 1
Battery | Charging capacity/mAh | Discharge capacity/mAh | Discharging efficiency/% | Battery | Charging capacity/mAh | Discharge capacity/mAh | Discharging efficiency/% |
A1 | 3804 | 3215 | 84.52 | A5 | 629 | 587 | 93.32 |
A2 | 3786 | 3106 | 82.04 | A6 | 632 | 582 | 92.09 |
A3 | 3874 | 3225 | 83.25 | A7 | 619 | 577 | 93.22 |
A4 | 3904 | 3279 | 83.99 | A8 | 640 | 599 | 93.59 |
DA1 | 3386 | 847 | 25.02 | DA3 | 558 | 261 | 46.77 |
DA2 | 3593 | 1693 | 47.12 | DA4 | 571 | 417 | 73.03 |
Table 2
Battery | Initial charge capacity/mAh | Discharge capacity/mAh first | Discharging efficiency/% | Capacity surplus ratio/% | Thickness/mm before circulation | Thickness/mm after circulation |
A9 | 984 | 980 | 99.59 | 62.7 | 5.3 | 6.2 |
A10 | 966 | 958 | 99.17 | 61.2 | 5.6 | 6.2 |
A11 | 974 | 969 | 99.49 | 60.7 | 5.4 | 6.1 |
A12 | 979 | 971 | 99.18 | 61.8 | 5.8 | 6.3 |
DA5 | 935 | 893 | 95.51 | 35.3 | 6.5 | 9.3 |
DA6 | 954 | 930 | 97.48 | 46.7 | 6.1 | 7.8 |
As can be seen from the test result of upper table 1, the charge-discharge performance of silicium cathode lithium-ion button battery provided by the invention is apparently higher than various battery of the prior art.As can be seen from the test result of upper table 2, silicium cathode lithium ion aluminum-shell battery of the present invention, has comparatively high charge-discharge performance, and after circulation, residual capacity is high, and before and after circulation, cell deformation is little, and battery life is longer.
Claims (6)
1. a silicon cathode lithium ion battery, comprise housing and be contained in battery core, the nonaqueous electrolytic solution in housing, battery core comprises positive pole, silicium cathode and the barrier film between positive pole and silicium cathode; Described nonaqueous electrolytic solution comprises lithium salts, nonaqueous solvents and additive, it is characterized in that, containing coke diene acid propyl diester in described additive, with the electrolyte of 100 weight portions for benchmark, the content of coke diene acid propyl diester is 0.1-10 weight portion, and described silicium cathode is the coated silicon nanowire material of silicon nanowire material or carbon.
2. silicon cathode lithium ion battery according to claim 1, is characterized in that, with the nonaqueous electrolytic solution of 100 weight portions for benchmark, the content of lithium salts is 1-10 weight portion, and the content of nonaqueous solvents is 80-98.9 weight portion.
3. silicon cathode lithium ion battery according to claim 1 and 2, is characterized in that, described lithium salts is selected from LiClO
4, LiPF
6, LiBF
4, LiAsF
6, LiSO
3f, LiCF
3sO
3in at least one.
4. silicon cathode lithium ion battery according to claim 1 and 2, is characterized in that, described nonaqueous solvents is selected from least one in vinyl carbonate, dimethyl carbonate, ethyl methyl carbonate, ethylene fluoride carbonic ether, diethyl carbonate.
5. silicon cathode lithium ion battery according to claim 1, is characterized in that, also containing pyrocarbonic acid diethyl ester and/or coke acid di-t-butyl ester in additive.
6. silicon cathode lithium ion battery according to claim 5, is characterized in that, with the nonaqueous electrolytic solution of 100 weight portions for benchmark, the content of pyrocarbonic acid diethyl ester is 0.1-10 weight portion, and the content of coke acid di-t-butyl ester is 0.1-10 weight portion.
Priority Applications (4)
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CN201110078105.5A CN102479973B (en) | 2010-11-24 | 2011-03-30 | Silicon cathode lithium ion battery |
EP11843832.4A EP2643879A4 (en) | 2010-11-24 | 2011-11-11 | Non-aqueous electrolyte and lithium-ion battery comprising the same |
PCT/CN2011/082113 WO2012068959A1 (en) | 2010-11-24 | 2011-11-11 | Non-aqueous electrolyte and lithium-ion battery comprising the same |
US13/301,821 US20120129054A1 (en) | 2010-11-24 | 2011-11-22 | Silicon anode lithium-ion battery |
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CN201010556261.3 | 2010-11-24 | ||
CN201010556261 | 2010-11-24 | ||
CN201110078105.5A CN102479973B (en) | 2010-11-24 | 2011-03-30 | Silicon cathode lithium ion battery |
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CN102479973B true CN102479973B (en) | 2015-02-04 |
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EP (1) | EP2643879A4 (en) |
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WO (1) | WO2012068959A1 (en) |
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2011
- 2011-03-30 CN CN201110078105.5A patent/CN102479973B/en not_active Expired - Fee Related
- 2011-11-11 EP EP11843832.4A patent/EP2643879A4/en not_active Withdrawn
- 2011-11-11 WO PCT/CN2011/082113 patent/WO2012068959A1/en active Application Filing
- 2011-11-22 US US13/301,821 patent/US20120129054A1/en not_active Abandoned
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
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US6174629B1 (en) * | 1999-09-10 | 2001-01-16 | Wilson Greatbatch Ltd. | Dicarbonate additives for nonaqueous electrolyte rechargeable cells |
CN101685875A (en) * | 2008-09-27 | 2010-03-31 | 财团法人工业技术研究院 | Lithium battery |
CN101684548A (en) * | 2009-03-05 | 2010-03-31 | 镇江科捷锂电池有限公司 | Method for preparing amorphous silicon nano wire and application thereof in cathode of lithium battery |
Also Published As
Publication number | Publication date |
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WO2012068959A1 (en) | 2012-05-31 |
EP2643879A1 (en) | 2013-10-02 |
US20120129054A1 (en) | 2012-05-24 |
EP2643879A4 (en) | 2014-07-23 |
CN102479973A (en) | 2012-05-30 |
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